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Membrane fouling and its control in

Water Science and Technology Vol 41 No 1011 pp 303308 2000 IWA Publishing and the authors
environmental applications
A.G. Fane, P. Beatson and H. Li
UNESCO Centre for Membrane Science and Technology, School of Chemical Engineering and Industrial
Chemistry, University of New South Wales, Sydney 2052, Australia

Abstract Fouling is an issue in the application of membranes to environmental management. This paper
describes recent developments in fouling analysis and membrane autopsy. Methods of fouling control are
described with examples of feed pretreatment, membrane selection, module design and selection and mode
of operation.
Keywords Membranes; fouling; environmental applications

Introduction
Membranes are important separation tchniques in environmental protection. They play a
key role in a wide range of situations including:
removal of contaminants from water; e.g. Desalination, water reclamation;
in recovery of values from effluents; e.g. whey processing;
in cleaner production by replacing less efficient processes or permitting system
integration; e.g. plating rinse water recycle.
In many actual or potential applications the biggest challenge is membrane fouling,
which increases costs and complicates operation. Table 1 summarises generic foulants in
membrane processing of aqueous feed and summarises some of the fouling control strate-
gies. This paper illustrates recent developments in fouling analysis and control based main-
ly on work in the UNESCO Centre for Membrane Science and Technology.

Fouling analysis
Whilst examination of membranes by EM is highly informative (see Autopsy below), there
is great advantage in application of non-invasive techniques capable of giving real-time
information about the fouling process. Two optical techniques will be described. Direct

Table 1 Foulants and foulant control

Process Foulant Control

RO General Hydrodynamics/shear
Inorganics (CaSO4, CaCO3 silica) Avoid solubility limit. Water pretreatment, pH 46, avoid
high recovery, additives (polyphosphates)
Organics Biological treatment, activated carbon, ozone
Colloids (<0.5 m) Coagulation filtration, microfiltration
Biological solids Chlorination/dechlorination, filtration, coagulation,
microfiltration
UF/MF General Hydrodynamics/shear (i.e. crossflow, backflushing, bubble
flow, sub-critical flux)
Hydrocarbons, surfactants Limit concentration in feed
Proteins Adjust pH and salts, hydrophilic and highly porous surface
Biological solids Hydrophilicity, porosity control
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A.G. Fane et al.

Figure 1 The critical flux versus Reynolds number for spacer filled channels and slit channel. The filtration
tests were conducted with 6.4 m latex suspensions, concentration 0.6 g/l. The spacers used were 0.71 mm
(28 mil) thick, with square net (S) of 4 mm diagonal, with orientation angles of 45 and 90 degrees to the
crossflow direction

observation through the membrane (DOTM) has recently been developed in our laboratory
(Li et al., 1998). This technique uses a microfiltration (MF) membrane which is transparent
when wet (anodised aluminium by Anopore, Whatman Ltd) in a crossflow test cell designed
to allow optical observation through the membrane of the feed/membrane interface. The
test loop provides independent control of crossflow rate and flux. Crucial information
obtained from this system includes (Li et al., 1998).
confirmation that for a feed with a size distribution the smaller particles deposit prefer-
entially (this is because hydrodynamic back-transport increases with particle size), and
the greater the crossflow the smaller the deposited particles;
surface coverage correlates well with observed increases in transmembrane pressure if
the particles are inert and well-defined; for feeds containing particles plus non-visible
species (cell debris etc.) the transmembrane pressure is greater than expected from
observed surface coverage;
a cake of inert species is readily swept from the membrane if the crossflow is increased or
the flux is reduced, whereas a cake of bacteria is incompletely released as slowly rolling
flocs (this is assumed due to the adhesive nature of bacterial EPS);
in spacer-filled channels the deposition tends to initiate in the centre of the cells between
the spacer filaments; this is the region of lowest velocity.
The DOTM technique also provides information on the critical flux, Jcrit, defined as the
flux at which deposition starts for a given feed and crossflow condition. Figure 1 illustrates
the relationship betwen Jcrit and channel Reynolds number for latex particles (6.4 mm). The
data show that Jcrit increases with Reynolds number and that channel spacers increase Jcrit.
Information such as this may be used in determining low fouling conditions (see below).
Another optical technique we are using involves direct observation of the surface of the
membrane (DOSM). (Chang and Fane, 2000). In this study we are examining the deposition
of biological solids on the outside of hollow fibres under conditions relevant to membrane
bioreactors.
Figure 2 shows the outer surface of the fibres after six hours of microfiltration of a yeast
suspension. From these images we can see a cake layer at initial fluxes of 30 and 15 l/m2 hr,
but not at 10 l/m2 hr. The feed contained air bubbles to reduce cake formation. From this
304 study the flux of 10 l/m2 hr appears to be below critical flux. We have used this technique to
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A.G. Fane et al.

Figure 2 Images taken after 6 hrs filtration of 5 g/l yeast suspensions with different initial fluxes (a) 30 1/m2
hr (b) 15 l/m2 hr (c) 10 l/m2 hr. Hollow fibres, bubbling axial flow (liquid 0.34 m/s, gas 0.19 m/s)

compare cake formation on axial or transverse flow hollow fibres, with and without bubble
flow.

Autopsy
Membrane autopsy is a valuable tool for fouling analysis. A range of techniques are avail-
able for autopsy to characterise the nature and location of the foulant. Autopsies of mem-
branes used in a Sewer Mining process involving MF and RO (Johnson et al., 1997) will be
used to illustrate this. In the process screened sewage was fed directly to a hollow fibre MF
membrane, and one of the issues was the presence of sulphur crystals due to the oxidation of
H2S. Examination of a hollow fibre in cross-section by EDAX mapping (Figure 3) indicat-
ed a predominantly surface deposition of sulphur, but also levels of sulphur above back-
ground within the membrane cross-section (Flood et al., 2000). This signified internal
fouling of the MF membrane and pointed to the need for changes to operating and cleaning
protocols.
The RO membranes in this process were also subject to sulphur particles as well as nutri-
ents in the feed. Complex fouling (biological plus depositional) was observed in the spiral-
wound RO elements, although operating and cleaning strategies were able to deal with this.
Elements from the head and tail of the array were autopsied (Beatson et al., submitted).
Figure 4 shows the non-uniform distribution of foulant on a single membrane leaf taken
from the first element in the array. Based on dry weight and elemental sulphur assays the
greatest deposition was on the left edge of the sheet, near the entry to the feed channels. The
distribution of wet weight corresponded to the expected flux distribution (highest in the top
left corner, lowest in the bottom right corner). Distribution of bacteria showed a similar
broad trend, but tended to be more patchy. The observations have implications for how we
design and operate spiral would modules (Fane et al., 1999).

Fouling control
The strategies for fouling control can be characterised by (i) feed pretreatment (ii) mem-
brane selection (iii) module design and selection, and (iv) mode of operation. Each of these
strategies will be illustrated and discussed.

Feed pretreatment
An example which illustrates the importance of pretreatment is water reclamation by RO
from sewage effluent. In the autopsy section (above) the use of MF as a pretreatment to RO 305
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Figure 3 Cryosection (4 m thick) of MF hollow fibre, SEM image. EDX was used to locate sulfur foulants
in this section, intensity of sulfur K X-ray emissions was measured at 512 points along a transect of the fibre
wall (below). Although the most intense signal locates most sulfur at the feed surface (F), it appears smaller
amounts have deposited deeper in the matrix, when compared to the background level. L=lumen surface.
Scale bar=50 microns. The fibres are composed of polypropylene and have no intrinsic sulfur signal

Figure 4 Distribution of foulants mapped over a single unrolled sheet of RO membrane. The membrane
area is marked by a 10 cm grid, the sheet is oriented so that the permeate collector tube is at top, and feed
came from the left edge. Above left: Wet weight of foulant, milligrams per square centimetre. Above right: Dry
weight. Below left: Sulfur crystal deposition. Below right: Bacterial numbers, cells per square centimetre.
Measurements were not made close to the edge due to glue lines, and drying caused by partial drainage of
306 the element prior to autopsy
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is described for a raw (screened) sewage reclamation process. The MF is clearly an essen-
tial feed pretreatment. For secondary effluent reclamation MF (or UF) is also a preferred
pretreatment since it significantly reduces colloidal and biological fouling of the RO. The
process whereby MF delays biofouling of the RO is of interest. We have examined the MF
of bacterial suspensions through 0.2 m MF membranes (Sadr. Ghayeni et al., 1999). Our
studies show that marine bacteria SW8 and sewage treatment bacteria at 106 to 107 cells/ml

A.G. Fane et al.

were removed with a log removal of 3.5 to 4.0 based on total counts, and in terms of cultur-
able counts the removal was complete, i.e. no cells in the permeate could be cultured. It is
believed that passage through the MF membranes injures the bacteria (they showed some
respiratory activity as determined by CTC uptake). Provided they are swept through the RO
system these bacteria would be unlikely to contribute significantly to biofouling. The fact
that biofouling occurs is probably due to isolated bioadhesion followed by colonisation and
proliferation on the RO surface.

Membrane selection
Membrane characteristics have a strong influence on propensity to fouling. Relevant prop-
erties are porosity characteristics, surface charge, hydrophilicity/phobicity and rugosity. In
the context of water reclamation by RO we have examined the relationship between initial
bioadhesion of sewage treatment bacteria (three isolates) and membrane properties (Sadr.
Ghayeni et al., 1998). No single characteristic could be unequivocally correlated with
bioadhesion. For example as shown in Table 2 only one out of three isolates showed
increased bioadhesion as contact angle increased, the other two showed no trend. In some of
our tests bacteria adhered as aggregates rather than as individuals, and the greatest aggrega-
tive adhesion appeared to occur on the roughest membrane surface. This may be of interest
given developments in RO membranes with extended surfaces.

Module design and selection

Spiral wound modules are popular because they provide a high surface area/volume.
Furthermore feed-side spacers are needed to maintain channel geometry, reduce concentra-
tion polarisation of macrosolutes, increase critical flux of particulates (Figure 1) and reduce
the rate of fouling of species such as whey proteins (Table 3 data from Da Costa et al.,
1993). On the other hand autopsies in our laboratory of spiral-wound modules treating
feeds containing substantial bacterial floc revealed excessive fouling deposits within the
spiral mesh. Under these conditions a more open spacer design may be appropriate
(Schwinge et al., 2000), or an open channel tubular module.

Mode of operation
These are significant opportunities to alleviate fouling by mode of operation (Table 1). One
method of interest is to identify the critical flux (see Figure 1) and aim to operate below this

Table 2 Initial bioadhesion of bacteria (three isolate from sewage treatment effluent) on different RO
membranes effect of contact angle

105 Bacterial cell per cm2

Contact angle 20 55 65 70 Trend

PP1* >50 >50 No

PA2 3.59.0 2.03.0 ~9.0 0.92.0 No
FP3 0.91.5 ~3.5 ~15.0 Yes

*Isolate identification 307

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Table 3 Fouling resistances for UF of whey (5 g/l) at 300 kPa in a spacer-filled channel

Solute and fouling resistance1013 (m1)

Spacer 0 mins 100 mins 300 mins

None 4 6 >11
UF4 1.6 2.0 2.5
A.G. Fane et al.

80 MIL-2 0.7 0.8 1.0

value. This approach is discussed in Cho et al. (1999), where Jcrit was identified as the flux
at which P(TM) started to rise substantially. For a multi component system this protocol may
have difficulties. As described in Cho et al. (1999) crossflow MF of MLSS below apparent Jcrit
showed a low P(TM) for an initial 20 to 30 hr period followed by a gradually then more rapid-
ly increasing P. This suggests that the Jcrit asessment identified the major cake forming
species (i.e. biomas floc) but not the low concentration of other species that slowly foul due to
transport into the pores and internal deposition. To overcome this type of fouling it may be nec-
essary to adopt other operational strategies, such as bubbling or rapid back pulsing, or employ
different membranes (smaller pores, etc) less susceptible to the trace foulants. Ths illustrates
that optimal performance may require attention to several fouling control strategies.

Conclusions
Environmental applications of membranes frequently lead to fouling. Fundamental studies
of membrane/feed interactions as well as membrane autopsies provide insights into fouling
mechanisms. The control of fouling can usually be achieved, but needs attention to feed
pretreatment, membrane and module selection and operating strategies.

Acknowledgements
The authors thank the Australia Research Council for supporting much of the work reported
here. The input of S. Chang and S.B. Ghayeni is gratefully acknowledged.

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